H2S 和 CO2 一步协同转化为合成气和硫磺,不仅实现了无害化处理,还能产生有价值的化学品,是废气升级再造的理想策略。然而,由于 H2S 和 CO2 的动力学惯性和高热力学稳定性,反应过程并未得到足够的重视。由于其非平衡特性,非热等离子体在增强转化过程中比热过程具有优势。在此,展示了一种由 Zn-Mo/Al2O3 催化剂偶联的非热等离子体新方法,用于同时转化 H2S 和 CO2。此外,与单组分催化剂(ZnS/Al2O3 和 MoS2/Al2O3)相比,具有不同 Zn/Mo 比例的 Zn-Mo/Al2O3 催化剂具有优异的催化性能。特别是,ZM(4/4) 催化剂显示出 H2S 的完全转化和大约 62% 的 CO2 转化,具有 0.95 mmol/kJ 的最高能效和 120 h 的长期稳定性。同时,通过原位直读光谱揭示了非热等离子体与催化之间的协同反应机理。本研究为等离子体催化法高效转化H2S-CO2酸性废气的催化剂设计提供了新的策略,并强调了Zn-Mo/Al2O3催化剂与非热等离子体之间的协同作用,以促进催化性能。
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Upcycling acid waste gas containing H2S and CO2 into syngas and sulfur by non-thermal plasma coupled with Zn-Mo/Al2O3 catalyst
Synergistic conversion of H2S and CO2 into syngas and sulfur in one step, not only achieves harmless treatment, but also produces valuable chemicals, which is an ideal strategy for waste gas upcycling. Nevertheless, due to the kinetic inertia and high thermodynamic stability of H2S and CO2, the process of the reaction has not received enough attention. Non-thermal plasma has advantages over thermal processes in the process of enhanced conversion owning to its non-equilibrium properties. Herein, a novel method of non-thermal plasma coupled by Zn-Mo/Al2O3 catalyst was demonstrated for the simultaneous conversion of H2S and CO2. Furthermore, compared to the single component catalysts (ZnS/Al2O3 and MoS2/Al2O3), the Zn-Mo/Al2O3 catalysts with different Zn/Mo ratios had excellent catalytic performance. In particular, the ZM(4/4) catalyst showed complete conversion of H2S and approximately 62 % of CO2 conversion, with the highest energy efficiency of 0.95 mmol/kJ and 120 h long-term stability. Meanwhile, the mechanism of the synergistic reaction between non-thermal plasma and catalysis was revealed by means of in-situ optical emission spectrometry. This study offers a new strategy for catalyst design for the highly efficient conversion of H2S-CO2 acid waste gas via plasma-catalytic method, and highlights the synergy between Zn-Mo/Al2O3 catalyst and non-thermal plasma to promote catalytic performance.